Cheng Yuan , Lei Wang , Pan Zeng , Chen Cheng , Hongtai Li , Tianran Yan , Genlin Liu , Gang Zhao , Xin Ma , Ting-Shan Chan , Liang Zhang
{"title":"通过界面微环境调控引导锂硫电池的硫还原动力学","authors":"Cheng Yuan , Lei Wang , Pan Zeng , Chen Cheng , Hongtai Li , Tianran Yan , Genlin Liu , Gang Zhao , Xin Ma , Ting-Shan Chan , Liang Zhang","doi":"10.1016/j.ensm.2024.103622","DOIUrl":null,"url":null,"abstract":"<div><p>Catalytic conversion of lithium polysulfides (LiPSs) is considered as an effective avenue to suppress the shuttle effect of lithium-sulfur (Li-S) batteries, for which the interfacial microenvironment constructed by the interaction between electrocatalysts and LiPSs plays a pivotal role in modulating the sulfur reduction kinetics. However, most of previous reports mainly focused on modulating the band structure of electrocatalysts or LiPSs alone to enhance the catalytic activity rather than considering the interfacial microenvironment as a whole. Herein, we propose a binary descriptor composed of the energy difference between <em>d</em>-band of electrocatalysts and <em>p</em>-band of LiPSs (Δε<sub>M-S</sub>) and the antibonding filling degree (ε<sub>ABF</sub>), which capture the energy band contributions from both electrocatalysts and LiPSs, to reveal the influence of interfacial microenvironment on sulfur reduction kinetics. Among different designed electrocatalysts, NiO presents a moderate LiPSs anchoring capacity and rapid electron transfer kinetics owing to the optimal Δε<sub>M-S</sub> and decreased ε<sub>ABF</sub> after interacting with LiPSs, which lead to a robust interfacial microenvironment and thus guarantee a continuous catalytic conversion of LiPSs in the long-term cycling. Such a fundamental understanding of catalytic activity toward LiPSs from the viewpoint of interfacial microenvironment provides an alternative avenue for designing highly efficient electrocatalysts for Li-S batteries.</p></div>","PeriodicalId":306,"journal":{"name":"Energy Storage Materials","volume":null,"pages":null},"PeriodicalIF":18.9000,"publicationDate":"2024-07-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Steering sulfur reduction kinetics of lithium-sulfur batteries by interfacial microenvironment modulation\",\"authors\":\"Cheng Yuan , Lei Wang , Pan Zeng , Chen Cheng , Hongtai Li , Tianran Yan , Genlin Liu , Gang Zhao , Xin Ma , Ting-Shan Chan , Liang Zhang\",\"doi\":\"10.1016/j.ensm.2024.103622\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>Catalytic conversion of lithium polysulfides (LiPSs) is considered as an effective avenue to suppress the shuttle effect of lithium-sulfur (Li-S) batteries, for which the interfacial microenvironment constructed by the interaction between electrocatalysts and LiPSs plays a pivotal role in modulating the sulfur reduction kinetics. However, most of previous reports mainly focused on modulating the band structure of electrocatalysts or LiPSs alone to enhance the catalytic activity rather than considering the interfacial microenvironment as a whole. Herein, we propose a binary descriptor composed of the energy difference between <em>d</em>-band of electrocatalysts and <em>p</em>-band of LiPSs (Δε<sub>M-S</sub>) and the antibonding filling degree (ε<sub>ABF</sub>), which capture the energy band contributions from both electrocatalysts and LiPSs, to reveal the influence of interfacial microenvironment on sulfur reduction kinetics. Among different designed electrocatalysts, NiO presents a moderate LiPSs anchoring capacity and rapid electron transfer kinetics owing to the optimal Δε<sub>M-S</sub> and decreased ε<sub>ABF</sub> after interacting with LiPSs, which lead to a robust interfacial microenvironment and thus guarantee a continuous catalytic conversion of LiPSs in the long-term cycling. Such a fundamental understanding of catalytic activity toward LiPSs from the viewpoint of interfacial microenvironment provides an alternative avenue for designing highly efficient electrocatalysts for Li-S batteries.</p></div>\",\"PeriodicalId\":306,\"journal\":{\"name\":\"Energy Storage Materials\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":18.9000,\"publicationDate\":\"2024-07-04\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Energy Storage Materials\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S2405829724004483\",\"RegionNum\":1,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Energy Storage Materials","FirstCategoryId":"88","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S2405829724004483","RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Steering sulfur reduction kinetics of lithium-sulfur batteries by interfacial microenvironment modulation
Catalytic conversion of lithium polysulfides (LiPSs) is considered as an effective avenue to suppress the shuttle effect of lithium-sulfur (Li-S) batteries, for which the interfacial microenvironment constructed by the interaction between electrocatalysts and LiPSs plays a pivotal role in modulating the sulfur reduction kinetics. However, most of previous reports mainly focused on modulating the band structure of electrocatalysts or LiPSs alone to enhance the catalytic activity rather than considering the interfacial microenvironment as a whole. Herein, we propose a binary descriptor composed of the energy difference between d-band of electrocatalysts and p-band of LiPSs (ΔεM-S) and the antibonding filling degree (εABF), which capture the energy band contributions from both electrocatalysts and LiPSs, to reveal the influence of interfacial microenvironment on sulfur reduction kinetics. Among different designed electrocatalysts, NiO presents a moderate LiPSs anchoring capacity and rapid electron transfer kinetics owing to the optimal ΔεM-S and decreased εABF after interacting with LiPSs, which lead to a robust interfacial microenvironment and thus guarantee a continuous catalytic conversion of LiPSs in the long-term cycling. Such a fundamental understanding of catalytic activity toward LiPSs from the viewpoint of interfacial microenvironment provides an alternative avenue for designing highly efficient electrocatalysts for Li-S batteries.
期刊介绍:
Energy Storage Materials is a global interdisciplinary journal dedicated to sharing scientific and technological advancements in materials and devices for advanced energy storage and related energy conversion, such as in metal-O2 batteries. The journal features comprehensive research articles, including full papers and short communications, as well as authoritative feature articles and reviews by leading experts in the field.
Energy Storage Materials covers a wide range of topics, including the synthesis, fabrication, structure, properties, performance, and technological applications of energy storage materials. Additionally, the journal explores strategies, policies, and developments in the field of energy storage materials and devices for sustainable energy.
Published papers are selected based on their scientific and technological significance, their ability to provide valuable new knowledge, and their relevance to the international research community.